Enhanced Photocatalytic and Photoluminescence Properties Resulting from Type-I Band Alignment in the Zn2 GeO4/g-C3 N4 Nanocomposites
Autor(a) principal: | |
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Data de Publicação: | 2022 |
Outros Autores: | , , , , , , |
Tipo de documento: | Artigo |
Idioma: | eng |
Título da fonte: | Repositório Institucional da UNESP |
Texto Completo: | http://dx.doi.org/10.3390/catal12070692 http://hdl.handle.net/11449/240328 |
Resumo: | Well-defined Zn2 GeO4/g-C3 N4 nanocomposites with a band alignment of type-I were prepared by the ultrasound-assisted solvent method, starting from g-C3 N4 nanosheets and incorporating 0, 10, 20, and 40 wt% of Zn2 GeO4. In this study, we have investigated in-depth the photoluminescence emission and photocatalytic activity of these nanocomposites. Our experimental results showed that an increased mass ratio of Zn2 GeO4 to g-C3 N4 can significantly improve their photoluminescence and photocatalytic responses. Additionally, we have noted that the broadband photoluminescence (PL) emission for these nanocomposites reveals three electronic transitions; the first two well-defined transitions (at ca. 450 nm and 488 nm) can be attributed to π* → lone pair (LP) and π* → π transitions of g-C3 N4, while the single shoulder at ca. 532 nm is due to the oxygen vacancy (Vo) as well as the hybridization of 4s and 4p orbital states in the Zn and Ge belonging to Zn2 GeO4. These experimental findings are also supported by theoretical calculations performed under periodic conditions based on the density functional theory (DFT) fragment. The theoretical findings for these nanocomposites sug-gest a possible strain-induced increase in the Zn-O bond length, as well as a shortening of the Ge-O bond of both tetrahedral [ZnO4] and [GeO4] clusters, respectively. Thus, this disordered structure promotes local polarization and a charge gradient in the Zn2 GeO4/g-C3 N4 interface that enable an efficient separation and transfer of the photoexcited charges. Finally, theoretical results show a good correlation with our experimental data. |
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Enhanced Photocatalytic and Photoluminescence Properties Resulting from Type-I Band Alignment in the Zn2 GeO4/g-C3 N4 Nanocompositesband alignmentDFT calculationsg-C3 N4/Zn2 GeO4nanocompositesoptical and photocatalytic propertiesWell-defined Zn2 GeO4/g-C3 N4 nanocomposites with a band alignment of type-I were prepared by the ultrasound-assisted solvent method, starting from g-C3 N4 nanosheets and incorporating 0, 10, 20, and 40 wt% of Zn2 GeO4. In this study, we have investigated in-depth the photoluminescence emission and photocatalytic activity of these nanocomposites. Our experimental results showed that an increased mass ratio of Zn2 GeO4 to g-C3 N4 can significantly improve their photoluminescence and photocatalytic responses. Additionally, we have noted that the broadband photoluminescence (PL) emission for these nanocomposites reveals three electronic transitions; the first two well-defined transitions (at ca. 450 nm and 488 nm) can be attributed to π* → lone pair (LP) and π* → π transitions of g-C3 N4, while the single shoulder at ca. 532 nm is due to the oxygen vacancy (Vo) as well as the hybridization of 4s and 4p orbital states in the Zn and Ge belonging to Zn2 GeO4. These experimental findings are also supported by theoretical calculations performed under periodic conditions based on the density functional theory (DFT) fragment. The theoretical findings for these nanocomposites sug-gest a possible strain-induced increase in the Zn-O bond length, as well as a shortening of the Ge-O bond of both tetrahedral [ZnO4] and [GeO4] clusters, respectively. Thus, this disordered structure promotes local polarization and a charge gradient in the Zn2 GeO4/g-C3 N4 interface that enable an efficient separation and transfer of the photoexcited charges. Finally, theoretical results show a good correlation with our experimental data.Fundação de Amparo à Pesquisa do Estado de São Paulo (FAPESP)Conselho Nacional de Desenvolvimento Científico e Tecnológico (CNPq)Coordenação de Aperfeiçoamento de Pessoal de Nível Superior (CAPES)Nanotechnology and Computational Chemistry Laboratory Federal University of Technology—Paraná, PRInstitute of Science Technology and Innovation Federal University of Bahia, BADepartment of Materials Engineering Federal University of Rio Grande do Norte, RNModeling and Molecular Simulation Group São Paulo State University, SPDepartment of Applied Physics Institute for Complex Molecular Systems (ICMS) Eindhoven University of Technology, Postbus 513Department of Physics of Complex Systems Weizmann Institute of ScienceDepartment of Chemical Research Support Weizmann Institute of SciencePost-Graduation Program in Chemistry State University of Londrina, PRModeling and Molecular Simulation Group São Paulo State University, SPFAPESP: 2013/07296-2FAPESP: 2019/08928-9FAPESP: 2022/03959-6CNPq: 307213/2021-8CAPES: 88887.467334/2019-00Federal University of Technology—ParanáUniversidade Federal da Bahia (UFBA)Federal University of Rio Grande do NorteUniversidade Estadual Paulista (UNESP)Eindhoven University of TechnologyWeizmann Institute of ScienceUniversidade Estadual de Londrina (UEL)Suzuki, Victor Y.Amorin, Luis H. C.Fabris, Guilherme S. L. [UNESP]Dey, SwayandiptaSambrano, Julio R. [UNESP]Cohen, HagaiOron, DanLa Porta, Felipe A.2023-03-01T20:12:15Z2023-03-01T20:12:15Z2022-07-01info:eu-repo/semantics/publishedVersioninfo:eu-repo/semantics/articlehttp://dx.doi.org/10.3390/catal12070692Catalysts, v. 12, n. 7, 2022.2073-4344http://hdl.handle.net/11449/24032810.3390/catal120706922-s2.0-85132721351Scopusreponame:Repositório Institucional da UNESPinstname:Universidade Estadual Paulista (UNESP)instacron:UNESPengCatalystsinfo:eu-repo/semantics/openAccess2023-03-01T20:12:16Zoai:repositorio.unesp.br:11449/240328Repositório InstitucionalPUBhttp://repositorio.unesp.br/oai/requestopendoar:29462023-03-01T20:12:16Repositório Institucional da UNESP - Universidade Estadual Paulista (UNESP)false |
dc.title.none.fl_str_mv |
Enhanced Photocatalytic and Photoluminescence Properties Resulting from Type-I Band Alignment in the Zn2 GeO4/g-C3 N4 Nanocomposites |
title |
Enhanced Photocatalytic and Photoluminescence Properties Resulting from Type-I Band Alignment in the Zn2 GeO4/g-C3 N4 Nanocomposites |
spellingShingle |
Enhanced Photocatalytic and Photoluminescence Properties Resulting from Type-I Band Alignment in the Zn2 GeO4/g-C3 N4 Nanocomposites Suzuki, Victor Y. band alignment DFT calculations g-C3 N4/Zn2 GeO4 nanocomposites optical and photocatalytic properties |
title_short |
Enhanced Photocatalytic and Photoluminescence Properties Resulting from Type-I Band Alignment in the Zn2 GeO4/g-C3 N4 Nanocomposites |
title_full |
Enhanced Photocatalytic and Photoluminescence Properties Resulting from Type-I Band Alignment in the Zn2 GeO4/g-C3 N4 Nanocomposites |
title_fullStr |
Enhanced Photocatalytic and Photoluminescence Properties Resulting from Type-I Band Alignment in the Zn2 GeO4/g-C3 N4 Nanocomposites |
title_full_unstemmed |
Enhanced Photocatalytic and Photoluminescence Properties Resulting from Type-I Band Alignment in the Zn2 GeO4/g-C3 N4 Nanocomposites |
title_sort |
Enhanced Photocatalytic and Photoluminescence Properties Resulting from Type-I Band Alignment in the Zn2 GeO4/g-C3 N4 Nanocomposites |
author |
Suzuki, Victor Y. |
author_facet |
Suzuki, Victor Y. Amorin, Luis H. C. Fabris, Guilherme S. L. [UNESP] Dey, Swayandipta Sambrano, Julio R. [UNESP] Cohen, Hagai Oron, Dan La Porta, Felipe A. |
author_role |
author |
author2 |
Amorin, Luis H. C. Fabris, Guilherme S. L. [UNESP] Dey, Swayandipta Sambrano, Julio R. [UNESP] Cohen, Hagai Oron, Dan La Porta, Felipe A. |
author2_role |
author author author author author author author |
dc.contributor.none.fl_str_mv |
Federal University of Technology—Paraná Universidade Federal da Bahia (UFBA) Federal University of Rio Grande do Norte Universidade Estadual Paulista (UNESP) Eindhoven University of Technology Weizmann Institute of Science Universidade Estadual de Londrina (UEL) |
dc.contributor.author.fl_str_mv |
Suzuki, Victor Y. Amorin, Luis H. C. Fabris, Guilherme S. L. [UNESP] Dey, Swayandipta Sambrano, Julio R. [UNESP] Cohen, Hagai Oron, Dan La Porta, Felipe A. |
dc.subject.por.fl_str_mv |
band alignment DFT calculations g-C3 N4/Zn2 GeO4 nanocomposites optical and photocatalytic properties |
topic |
band alignment DFT calculations g-C3 N4/Zn2 GeO4 nanocomposites optical and photocatalytic properties |
description |
Well-defined Zn2 GeO4/g-C3 N4 nanocomposites with a band alignment of type-I were prepared by the ultrasound-assisted solvent method, starting from g-C3 N4 nanosheets and incorporating 0, 10, 20, and 40 wt% of Zn2 GeO4. In this study, we have investigated in-depth the photoluminescence emission and photocatalytic activity of these nanocomposites. Our experimental results showed that an increased mass ratio of Zn2 GeO4 to g-C3 N4 can significantly improve their photoluminescence and photocatalytic responses. Additionally, we have noted that the broadband photoluminescence (PL) emission for these nanocomposites reveals three electronic transitions; the first two well-defined transitions (at ca. 450 nm and 488 nm) can be attributed to π* → lone pair (LP) and π* → π transitions of g-C3 N4, while the single shoulder at ca. 532 nm is due to the oxygen vacancy (Vo) as well as the hybridization of 4s and 4p orbital states in the Zn and Ge belonging to Zn2 GeO4. These experimental findings are also supported by theoretical calculations performed under periodic conditions based on the density functional theory (DFT) fragment. The theoretical findings for these nanocomposites sug-gest a possible strain-induced increase in the Zn-O bond length, as well as a shortening of the Ge-O bond of both tetrahedral [ZnO4] and [GeO4] clusters, respectively. Thus, this disordered structure promotes local polarization and a charge gradient in the Zn2 GeO4/g-C3 N4 interface that enable an efficient separation and transfer of the photoexcited charges. Finally, theoretical results show a good correlation with our experimental data. |
publishDate |
2022 |
dc.date.none.fl_str_mv |
2022-07-01 2023-03-01T20:12:15Z 2023-03-01T20:12:15Z |
dc.type.status.fl_str_mv |
info:eu-repo/semantics/publishedVersion |
dc.type.driver.fl_str_mv |
info:eu-repo/semantics/article |
format |
article |
status_str |
publishedVersion |
dc.identifier.uri.fl_str_mv |
http://dx.doi.org/10.3390/catal12070692 Catalysts, v. 12, n. 7, 2022. 2073-4344 http://hdl.handle.net/11449/240328 10.3390/catal12070692 2-s2.0-85132721351 |
url |
http://dx.doi.org/10.3390/catal12070692 http://hdl.handle.net/11449/240328 |
identifier_str_mv |
Catalysts, v. 12, n. 7, 2022. 2073-4344 10.3390/catal12070692 2-s2.0-85132721351 |
dc.language.iso.fl_str_mv |
eng |
language |
eng |
dc.relation.none.fl_str_mv |
Catalysts |
dc.rights.driver.fl_str_mv |
info:eu-repo/semantics/openAccess |
eu_rights_str_mv |
openAccess |
dc.source.none.fl_str_mv |
Scopus reponame:Repositório Institucional da UNESP instname:Universidade Estadual Paulista (UNESP) instacron:UNESP |
instname_str |
Universidade Estadual Paulista (UNESP) |
instacron_str |
UNESP |
institution |
UNESP |
reponame_str |
Repositório Institucional da UNESP |
collection |
Repositório Institucional da UNESP |
repository.name.fl_str_mv |
Repositório Institucional da UNESP - Universidade Estadual Paulista (UNESP) |
repository.mail.fl_str_mv |
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1803650139165818880 |